硝酸生产尾气中NO x 和N2O联合脱除技术研究进展

doi:10.16085/j.issn.1000-6613.2022-1614

摘要/Abstract

摘要：

采用氨氧化法生产稀硝酸时会排放NO _x （NO和NO₂）和N₂O等有害气体，可导致光化学烟雾（NO _x ）、臭氧层消耗（NO _x 和N₂O）、全球变暖（N₂O）等环境问题，减少硝酸生产尾气中NO _x 和N₂O的排放势在必行。本文在分析硝酸生产过程中NO _x 和N₂O产生途径及减排措施的基础上，根据国内外研发和应用情况总结了联合脱除硝酸生产尾气中NO _x 和N₂O的主要技术路线，包括利用SCR催化剂同时催化NO _x 和N₂O还原和利用复合式催化剂同时催化NO _x 还原和N₂O分解等一段式工艺以及先催化N₂O分解后催化NO _x 还原、先催化NO _x 还原后催化N₂O还原和先催化NO _x 还原后催化N₂O分解等两段式工艺，分析了不同技术路线的原理、特点及面临的挑战。文中指出了一段式工艺主要存在N₂O净化性能有待提升的问题，两段式工艺中先催化NO _x 还原后催化N₂O分解的工艺在减少还原剂消耗量、促进N₂O去除等方面具有优势，未来需围绕同步降低SCR脱硝和N₂O分解所需温度、提高催化剂对共存气体（O₂、H₂O等）的耐受性等方面开展进一步研究。

关键词: 硝酸生产尾气, 氮氧化物, 温室气体, 选择性催化还原, N₂O分解, 催化剂

Abstract:

Harmful gases such as NO _x (NO and NO₂) and N₂O are emitted during the production of dilute nitric acid by ammonia oxidation, which can lead to environmental problems such as photochemical smog (NO _x ), ozone layer depletion (NO _x and N₂O), and global warming (N₂O). It is imperative to remove NO _x and N₂O from the tail gas of nitric acid production. After introducing the generation pathways and control measures of NO _x and N₂O during nitric acid production, we summarized the main technological routes for simultaneous removal of NO _x and N₂O from the tail gas according to the research, development and application situations, including one-stage processes such as simultaneous SCR of NO _x and N₂O, SCR of NO _x and decomposition of N₂O over a composite catalyst, and two-stage processes such as catalytic N₂O decomposition followed by SCR of NO _x, SCR of NO _x followed by SCR of N₂O, and SCR of NO _x followed by catalytic N₂O decomposition. The principles and characteristics of different technological routes were analyzed. It was pointed out that the one-stage processes face challenges of improving the purification performance toward N₂O. The two-stage process of SCR of NO _x followed by catalytic N₂O decomposition, has advantages of low consumption of reducing agent and high purification efficiency of N₂O. Further research should focus on lowering the temperatures of both SCR of NO _x and catalytic N₂O decomposition and improving the tolerance of catalysts to co-existing gases (O₂, H₂O, etc.).

Key words: tail gas of nitric acid production, nitrogen oxide, greenhouse gas, selective catalytic reduction (SCR), N₂O decomposition, catalysts

中图分类号:

李佳, 樊星, 陈莉, 李坚. 硝酸生产尾气中NO _x 和N₂O联合脱除技术研究进展[J]. 化工进展, 2023, 42(7): 3770-3779.

LI Jia, FAN Xing, CHEN Li, LI Jian. Research progress of simultaneous removal of NO _x and N₂O from the tail gas of nitric acid production[J]. Chemical Industry and Engineering Progress, 2023, 42(7): 3770-3779.

图/表 5

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尾气组成	体积分数/%
NO _x	0.01~0.35
N₂O	0.03~0.35
O₂	1~4
H₂O	0.3~2

尾气组成	体积分数/%
NO _x	0.01~0.35
N₂O	0.03~0.35
O₂	1~4
H₂O	0.3~2

催化剂体系	特点
锰氧化物基	低温（＜250℃）催化剂，改性后可进一步提高催化剂活性，耐硫性差，高温下N₂选择性明显下降
钒氧化物基	中低温（300~400℃）催化剂，耐硫耐水性能优异，操作温度窗口窄，高温下催化剂稳定性和选择性差，主要用于工业尾气脱硝
铜分子筛	中低温（＜400℃）催化剂，低温活性和N₂选择性优异，高温水热稳定性较差，适用于低硫环境下的SCR脱硝，如汽车尾气脱硝
铁分子筛	高温（＞400℃）催化剂，高温活性和N₂选择性优异，操作温度窗口宽，水热稳定性好，适用于低硫环境下的SCR脱硝，如电厂尾气脱硝

催化剂体系	特点
锰氧化物基	低温（＜250℃）催化剂，改性后可进一步提高催化剂活性，耐硫性差，高温下N₂选择性明显下降
钒氧化物基	中低温（300~400℃）催化剂，耐硫耐水性能优异，操作温度窗口窄，高温下催化剂稳定性和选择性差，主要用于工业尾气脱硝
铜分子筛	中低温（＜400℃）催化剂，低温活性和N₂选择性优异，高温水热稳定性较差，适用于低硫环境下的SCR脱硝，如汽车尾气脱硝
铁分子筛	高温（＞400℃）催化剂，高温活性和N₂选择性优异，操作温度窗口宽，水热稳定性好，适用于低硫环境下的SCR脱硝，如电厂尾气脱硝

项目	联合脱除工艺
项目	SCR催化剂同时催化 NO _x 和N₂O还原	复合式催化剂同时催化 NO _x 还原和N₂O分解	先催化N₂O分解，后催化NO _x 还原	先催化NO _x 还原，后催化N₂O还原	先催化NO _x 还原，后催化N₂O分解
工艺类型	一段式	一段式	两段式	两段式	两段式
布设位置	尾气膨胀机之前	尾气膨胀机之前	尾气膨胀机之前	尾气膨胀机之前	尾气膨胀机之后
工艺特点	可同步脱除NO _x 和N₂O，工艺布置紧凑	可同步脱除NO _x 和N₂O，工艺布置紧凑	可利用NO _x 对N₂O分解的促进作用	适用范围广，脱除效率高	对硝酸生产工艺无影响，净化装置安装限制小
开发阶段	尚在研究	尚在研究	已有应用	已有应用	尚在研究
催化剂	Fe-beta	Bi-Ni/V₂O₅-WO₃/TiO₂	Fe-分子筛	Fe-分子筛	V₂O₅/Al₂O₃（NO _x 还原）、改性Co₃O₄（N₂O分解）
反应条件	367μL/L NO _x +1645μL/L N₂O+2012μL/L NH₃+1.56% O₂+N₂（平衡）、空速8200h^-1、温度354~373℃	250μL/L NO+125μL/L N₂O+250μL/L NH₃+3% O₂+N₂（平衡）、空速45000h^-1、温度390℃	Borealis AG硝酸厂、1200t/d、温度425~520℃	Abu Qir Fertilizer硝酸厂、1830t/d、温度330~520℃	700~1500μL/L NO _x +900~1200μL/L N₂O+700~1500μL/L NH₃+1.9%~4.5% O₂+N₂（平衡）、NO _x 还原段空速9664h^-1、温度220~240℃、N₂O分解段空速7667h^-1、温度230~260℃
脱除效率或排放浓度
NO _x	＞96%	90%	出口浓度5~10μL/L	出口浓度约1μL/L	＞98%（模拟结果）
N₂O	＞96%	72%	＞98%	＞99%	＞98%（模拟结果）
参考文献	[43]	[44]	[12]	[12]	[7]
发展方向	改善催化剂低温活性（尤其是催化N₂O还原/分解的活性），提高催化剂抗共存气体干扰性		拓宽催化剂活性温度窗口		降低N₂O分解所需温度，提高工艺净化实际尾气的性能

硝酸生产尾气中NO _x 和N₂O联合脱除技术研究进展

Research progress of simultaneous removal of NO _x and N₂O from the tail gas of nitric acid production

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